Year of Publication

2019

Degree Name

Doctor of Philosophy (PhD)

Document Type

Doctoral Dissertation

College

Engineering

Department

Chemical and Materials Engineering

First Advisor

Dr. J. Zach Hilt

Abstract

Iron oxide nanoparticles (IONPs) have been widely studied for a variety of applications, from biomedical applications (e.g., cell separation, drug delivery, contrast agent for magnetic resonance imaging and magnetically mediated energy delivery for cancer treatment) to environmental remediations (e.g., heavy metal removal and organic pollutants degradation). It has been demonstrated that IONPs can induce the production of reactive oxygen species (ROS) via Fenton/Haber-Weiss reactions which has been shown to be one of the key underlying mechanisms of nanoparticles toxicity. This inherent toxicity of nanoparticles has been shown to enhance the efficacy of traditional cancer therapies such as chemotherapy and radiation. In addition, the generation of ROS induced by IONPs has been also studied as advanced oxidation processes (AOP) for wastewater treatment. Recent research has also shown that exposure to an alternating magnetic field can significantly enhance the generation of ROS induced by IONPs. Moreover, the coatings of IONPs play an important role on the surface reactivity of nanoparticles since it can prevent the generation of ROS via Fenton chemistries at the surface of the nanoparticles.

In this work, co-precipitated IONPs were functionalized with small molecules including citric acid, sodium phosphate, amino silane and dopamine. The impact of coating on surface reactivity of the as-synthesized particles was studied using methylene blue dye degradation assay under AMF exposure. With the coatings of these small molecules, the IONPs induced ROS generation was significantly decreased because of the dense surface coverage. To study the effect of polymeric coatings, a degradable poly (beta amino ester) (PBAE) polymer coating was synthesized with dopamine as an anchor to bind to nanoparticles. The surface reactivity of the particles was expected to be recovered once the polymer coating was degraded. Furthermore, the impact of non-degradable PEG-based polymer coating on surface reactivity via ROS generation was also investigated using methylene blue decolorization assay with the presence of AMF. The retention of surface reactivity of PEG-based polymer coated IONPs shows promise for cancer treatment.

The application of IONPs as heterogeneous catalyst for organic contaminant degradation was investigated. Bisphenol A (BPA) was used as a model compound, and Fenton reactions were induced by IONPs with the presence of hydrogen peroxide and hydroxylamine as well as alternating magnetic field exposure. The kinetics of BPA degradation under water bath and AMF exposure at 37oC was also studied, and the results showed potential applications of IONPs for organic pollutants remediation.

Digital Object Identifier (DOI)

https://doi.org/10.13023/etd.2019.296

Funding Information

Vietnam Education Foundation

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